This first of three reports on a computational study of a drop-laden temporal mixing layer presents the results of direct numerical simulations (DNS) of well-resolved flow fields and the derivation of the large-eddy simulation (LES) equations that would govern the larger scales of a turbulent flow field. The mixing layer consisted of two counterflowing gas streams, one of which was initially laden with evaporating liquid drops. The gas phase was composed of two perfect gas species, the carrier gas and the vapor emanating from the drops, and was computed in an Eulerian reference frame, whereas each drop was tracked individually in a Lagrangian manner. The flow perturbations that were initially imposed on the layer caused mixing and eventual transition to turbulence. The DNS database obtained included transitional states for layers with various liquid mass loadings. For the DNS, the gas-phase equations were the compressible Navier-Stokes equations for conservation of momentum and additional conservation equations for total energy and species mass. These equations included source terms representing the effect of the drops on the mass, momentum, and energy of the gas phase. From the DNS equations, the expression for the irreversible entropy production (dissipation) was derived and used to determine the dissipation due to the source terms. The LES equations were derived by spatially filtering the DNS set and the magnitudes of the terms were computed at transitional states, leading to a hierarchy of terms to guide simplification of the LES equations. It was concluded that effort should be devoted to the accurate modeling of both the subgridscale fluxes and the filtered source terms, which were the dominant unclosed terms appearing in the LES equations.